CN104152174B - A kind of naphtha catalytic cracking method - Google Patents
A kind of naphtha catalytic cracking method Download PDFInfo
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- CN104152174B CN104152174B CN201310177863.1A CN201310177863A CN104152174B CN 104152174 B CN104152174 B CN 104152174B CN 201310177863 A CN201310177863 A CN 201310177863A CN 104152174 B CN104152174 B CN 104152174B
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Abstract
The invention discloses a kind of naphtha catalytic cracking method, the method is included under catalytic pyrolysis condition, under the existence of promoter component, feed naphtha is contacted and reacted with catalytic cracking catalyst, thereby improve naphtha catalytic cracking conversion ratio and productivity of low carbon olefin hydrocarbon. When taking straight-run naphtha as raw material, compared with not injecting the comparative example of promoter component under equivalent responses condition, to introduce after promoter component, conversion ratio and the productivity of low carbon olefin hydrocarbon of raw material significantly improve, and can improve respectively more than 15 and 17 percentage points.
Description
Technical field
The present invention relates to a kind of naphtha catalytic cracking method.
Background technology
The low-carbon alkene such as ethene, propylene is important basic organic chemical industry raw material, has the foot of act in the national economic developmentThe status of weight. At present, in world wide, the production of low-carbon alkene mainly adopts the tubular type taking light hydrocarbons such as naphthas as raw materialStove steam splitting process, reaction need to be carried out with having under a large amount of steam participation conditions by high temperature conventionally more than 800 DEG C, has energy consumptionHigh, CO2Large and the propylene of discharge capacity with weight ethylene than low (being conventionally about 0.4～0.6), be difficult to meet the day of market to propyleneThe technology limitations such as benefit increased requirement. In contrast to this, due to the intervention of catalyst, naphtha catalytic cracking can be anti-what relatively relaxAnswer under condition and produce low-carbon alkene, the energy consumption of reaction and CO2Discharge capacity is lower; And this process is mainly entered by carbonium ion mechanismRow reaction, in gaseous product, propylene, with weight ethylene than high, is expected to meet growing propylene demand, therefore naphtha catalysisMore attractive and the competitiveness of producing low-carbon olefins by cracking.
CN102295510A discloses a kind of naphtha and has been catalytically conveted to the method for low-carbon alkene, and the method comprises naphthaContact and react with catalyst with in bed tandem reactor at riser, generate product, form carbon deposited catalyst simultaneously; WillCarbon deposited catalyst part after stripping is returned to epimere bed reactor, and part enters regenerator regeneration, the catalyst after regenerationEnter hypomere riser reactor.
US20070083071A1 discloses a kind of method of naphtha catalytic cracking production ethene, propylene, and the method comprisesNaphtha is contacted with ZSM-5 molecular sieve catalyst in fixed bed or fluidized-bed reactor and anti-under catalyticing conversioning conditionShould; Product is separated into C2～C3 alkane, C2～C3 alkene and three kinds of logistics of C4+ hydrocarbon through series of process; C2～C3 alkaneReturn to tube cracking furnace and carry out thermal cracking; C4+ logistics is returned and in above-mentioned fixed bed or fluidized-bed reactor, is carried out catalytic pyrolysis.
CN101462916A discloses and has a kind ofly produced the method for low-carbon alkene by petroleum hydrocarbon catalytic pyrolysis, the method comprise byPetroleum hydrocarbon carries out catalytic dehydrogenation under catalytic dehydrogenation catalyst existence and catalytic dehydrogenation condition, and then gained catalytic dehydrogenation is producedThing carries out catalytic cracking reaction under catalytic cracking catalyst existence and catalytic pyrolysis condition.
Naphtha is to be made up of the shorter C4～C12 hydro carbons of chain length, because the alkane molecule as its key component is difficult forIn catalyst surface absorption, and be difficult to by direct activation, therefore the conversion ratio of naphtha catalytic cracking and productivity of low carbon olefin hydrocarbon are logicalOften lower. The naphtha catalytic cracking method of mentioning in above-mentioned patent application adopts raw material systemic circulation ratio or the pre-dehydrogenating technology of catalysisAlthough promoted naphtha pyrolysis to generate low-carbon alkene, naphtha conversion ratio and productivity of low carbon olefin hydrocarbon are still lower, and have energyConsume high, complicated operation and the high deficiency of cost of investment.
Summary of the invention
The object of the invention is for overcome existing naphtha catalytic cracking method exist naphtha conversion ratio lower andThe lower defect of productive rate of low-carbon alkene, provides a kind of naphtha catalytic cracking method.
The invention provides a kind of naphtha catalytic cracking method, the method comprises: under catalytic pyrolysis condition, promotingUnder the existence of agent component, feed naphtha is contacted with catalytic cracking catalyst, wherein, described promoter component is and described stoneCerebrol raw material is compared and can on the surface of described catalytic cracking catalyst, preferentially be adsorbed and/or the material of preferential reaction.
The present inventor studies discovery by experiment, in naphtha catalytic cracking process, will be easy at catalystThe promoter component of adsorption and/or reaction is introduced in reaction system, utilize preferential absorption promoter component self and/orInteraction between the carbonium ion that its preferential reaction generates and naphtha hydrocarbon molecules can promote and/or cause stone indirectlyCerebrol hydrocarbon molecules is in absorption and the activation of catalyst surface, thus the catalytic cracking reaction of promotion naphtha, and then improve lowCarbon olefin (as ethene and propylene) productive rate, and reduce the productive rate of the low value such as methane, ethane product.
Other features and advantages of the present invention are described in detail the detailed description of the invention part subsequently.
Brief description of the drawings
Accompanying drawing is to be used to provide a further understanding of the present invention, and forms a part for description, with tool belowBody embodiment one is used from explanation the present invention, but is not construed as limiting the invention. In the accompanying drawings:
Fig. 1 is that equipment and the logistics that described naphtha catalytic cracking method of the present invention adopts flows to schematic diagram.
Detailed description of the invention
Naphtha catalytic cracking method according to the present invention comprises: under catalytic pyrolysis condition, in promoter componentExistence under, feed naphtha is contacted with catalytic cracking catalyst, wherein, described promoter component is former with described naphthaMaterial is compared and can on the surface of described catalytic cracking catalyst, preferentially be adsorbed and/or the material of preferential reaction.
In described method provided by the invention, with respect to the consumption of the described feed naphtha of 100 weight portions, described shortThe consumption that enters agent component can be 0.01-30 weight portion, is preferably 0.05-15 weight portion.
What in the present invention, described promoter component can be for various routines can be in institute compared with described feed naphthaThe material of stating preferential absorption on the surface of catalytic cracking catalyst and/or preferential reaction can be for example petroleum hydrocarbon oil, mineralAt least one in oil, artificial oil, bio-oil and organic oxygen-containing compound. Described oil hydrocarbon ils can be selected from C4～C12 and heat up in a steamerPoint, AGO (atmospheric gas oil), vacuum gas oil (VGO), coker gas oil, deasphalted oil, hydrogenation tail oil, reduced crude, decompression residuum and crude oilIn at least one. Described mineral oil can be selected from least one in liquefied coal coil, tar sand oil and shale oil. Described artificial oilIt can be the synthetic distillate obtaining of at least one process Fischer-Tropsch by coal, natural gas or pitch. Described bio-oil is passableBe selected from least one in vegetable fat, animal fat and microbial grease. Described organic oxygen-containing compound can be selected from C1～At least one in ketone, the aldehyde of C1～C36 and the carboxylic acid of C1～C36 of the alcohol of C5, the ether of C2～C6, C3～C5. Alcohol for example canThink at least one in methyl alcohol, ethanol and ethylene glycol. Ether can be for example dimethyl ether and/or ether. Ketone can be for example thirdKetone. Aldehyde can be for example at least one in formaldehyde, octanal, capraldehyde and lauric aldehyde. Carboxylic acid can be for example the fat of C1～C36At least one in acid and aphthenic acids.
In described method provided by the invention, described catalytic pyrolysis condition can comprise: temperature is 500-750 DEG C, excellentElect 540-700 DEG C as, more preferably 560-690 DEG C; Time is 0.2-10 second, is preferably 0.5-5 second; Agent weight of oil is than being 6-80, be preferably 10-60, more preferably 20-40. Described dose of weight of oil is than the weight that refers to catalytic cracking catalyst and feed naphthaAmount ratio.
In described method provided by the invention, recycle ratio can be 0.05-0.9, is preferably 0.1-0.6, more preferably0.1-0.4. Described recycle ratio refers to the ratio of the above cut weight flow of C4 returned of circulation and fresh feed weight flow.
In described method provided by the invention, in naphtha catalytic cracking process, conventionally need injected water steam. Water steamsThe weight ratio of the consumption of gas and feed naphtha can be 0.05-1:1, is preferably 0.1-0.6:1.
In the present invention, described catalytic cracking catalyst can be the conventional various catalyst that use in this area, for example, and instituteState catalytic cracking catalyst and can contain molecular sieve, heat-resistant inorganic oxide and optional clay. In described catalytic pyrolysis catalysisIn agent, taking the gross weight of described catalytic cracking catalyst as benchmark, the content of described molecular sieve can be 5-60 % by weight, preferablyFor 10-55 % by weight; The content of described heat-resistant inorganic oxide is 40-95 % by weight, is preferably 45-80 % by weight; Described clayContent is 0-70 % by weight, is preferably 10-45 % by weight. Described molecular sieve can be the conventional molecular sieve using in this area, for exampleCan be for being selected from ZSM molecular sieve, ZRP molecular sieve, ZSP molecular sieve, SAPO molecular sieve, beta-molecular sieve and above-mentioned molecular sieve processAt least one in the molecular sieve that physics and/or chemical method obtain after processing. Described heat-resistant inorganic oxide is not specialLimiting, for example, can be silica and/or alundum (Al2O3). Described clay can be for example that kaolin is (as many water Gao LingSoil), at least one in ball clay, imvite, diatomite, tired de-soil, hydrotalcite, bentonite and laminated clay column.
In the present invention, described naphtha catalytic cracking method can comprise urging of reactor, settler and stripperChange in cracker and implement, feed naphtha and catalytic cracking catalyst carry out catalytic cracking reaction in described reactor,Enter in settler and carry out sedimentation separation to the mixture that contains oil gas and carbon deposited catalyst, isolated carbon deposited catalyst entersIn stripper, carry out stripping, the regenerated catalyst obtaining through stripping turns back in reactor by regenerated catalyst lineRecycle. Described promoter component can be in described regenerated catalyst line, described reactor, described settler and instituteAt least one place stating in stripper adds. Under preferable case, described promoter component adds in reactor. When described promoterWhen component is injected by multiple different positions simultaneously, each position can be to measure arbitrarily injection promoter component, for example eachThe amount that promoter component is injected in individual position can account for the 1-90% that needs the promoter component total amount of injecting.
Fig. 1 is that while adopting riser reactor, promoter component and feed naphtha are mixed together from riser bottomSchematic flow sheet while entering reactor use. In the method shown in this figure, the regenerated catalyst of heat is carried through regenerated catalystPipeline 10 enters the bottom of riser reactor 4, and accelerates to upper reaches under the effect of the pre-lift medium being injected by pipeline 1Moving. Feed naphtha after preheating presses one through pipeline 2 and from the atomizing steam of pipeline 4 with from the promoter component of pipeline 3After certainty ratio is mixed, injecting lift pipe reactor 4 contacts, reacts with thermocatalyst in the situation that promoter component exists, anti-Answering temperature is 500 DEG C～750 DEG C, and the reaction time is 0.2～10 second, and the weight ratio of catalyst and feed naphtha is 6～80. InsteadAnswer the mixture of oil gas and catalyst to enter settler 7 after riser goes upward to leg outlet place, in the interior reaction of settler 7The catalyst separation of oil gas and carbon deposit, reaction oil gas is sent into subsequent separation system through pipeline 8 and is further separated and obtain object productEthene, propylene etc. and (in figure, not marking) such as gasoline, diesel oil, heavy oil. After reaction, the catalyst of carbon deposit enters stripper 6, strippingSteam injects through pipeline 5, with the catalyst counter current contacting of carbon deposit, by the reaction oil gas entrained catalyst of carbon deposit as much as possibleStripping is clean. Catalyst after stripping is sent into regenerator 12 coke burning regenerations through reclaimable catalyst feed-line 9. Oxygen-containing gas is as skyGas injects regenerator 12 through pipeline 11, and regenerated flue gas is drawn through pipeline 13. Catalyst after regeneration is through regenerated catalystLine 10 returns to riser reactor 4 and recycles.
Compared with prior art, described method tool provided by the invention has the following advantages:
Compared with the naphtha catalytic cracking technology operating with existing employing raw material systemic circulation ratio, naphtha provided by the inventionThe method of catalytic pyrolysis increased low carbon olefine output adopts the promoter component that possesses preferential absorption and/or preferential reaction indirectly to promoteNaphtha hydrocarbon molecules, in absorption and the activation of catalyst surface, is improving naphtha catalytic cracking conversion ratio and low-carbon alkene productWhen rate, also reduce energy consumption of reaction.
Promoter component of the present invention is the normally used material in refinery, and existing apparatus is slightly done to changeImplement method of the present invention, therefore the present invention can significantly improve naphtha catalytic cracking by simple, cheap modeConversion ratio and productivity of low carbon olefin hydrocarbon. From embodiment, under identical reaction condition, adopt method processing provided by the inventionWhen naphtha, the conversion ratio of raw material can improve more than 17 percentage points, and productivity of low carbon olefin hydrocarbon can improve more than 20 percentage points.
The invention will be further described by the following examples.
In following examples and comparative example, feed naphtha used is straight-run naphtha, and its character is as shown in table 1.
The catalyst using in following examples and comparative example contains and has MFI structure molecular screen and FAU structure is dividedThe mixed molecular sieve catalyst of son sieve. Wherein, there is MFI structure molecular screen and FAU structure molecular screen by SinopecCatalyst asphalt in Shenli Refinery of limited company industrial production, trade names are respectively ZRP-1(SiO2/Al2O3=30, rare earth containsAmount RE2O3=2.0 % by weight) and DASY(lattice constant be 2.445～2.448 nanometers). Used catalyst composed as follows: to urgeThe gross weight of agent is benchmark, and containing ZRP-1 molecular sieve, the 2 % by weight DASY molecular sieves of 18 % by weight, surplus is heat-resisting inorganic oxideThing, its main character is listed in table 3.
Embodiment 1
The present embodiment is used for illustrating described naphtha catalytic cracking method of the present invention.
On small fixed flowing bed device, adopt intermittently operated, straight-run naphtha, as the normal pressure slag of promoter componentOil and atomizing steam enter bottom fluidized-bed reactor by feed nozzle after preheating furnace is heated to 380 DEG C of left and right, with heatCatalytic conversion reaction is carried out in catalyst contact. After product and catalyst separation, enter piece-rate system, product is furtherBe separated into gaseous product and product liquid. After reaction finishes, enter the stripping stage, gone out on reclaimable catalyst to inhale by steam strippingAttached hydro carbons. In the backward reactor of stripping, passing into oxygen-containing gas regenerates. The main operating condition of experiment and the results are shown in table4。
Comparative example 1
According to the method for embodiment 1, described straight-run naphtha raw material is carried out to catalytic pyrolysis, difference is not add shortEnter agent component. The main operating condition of experiment and the results are shown in table 4.
Comparative example 2
According to the method for embodiment 1, described straight-run naphtha raw material is carried out to catalytic pyrolysis, difference is not add shortEnter agent component, at the higher water injection rate of employing compared with embodiment 1, the weight ratio of steam and feed naphtha is 0.8. ExperimentMain operating condition and the results are shown in table 4.
Embodiment 2
The present embodiment is used for illustrating described naphtha catalytic cracking method of the present invention.
According to the method for embodiment 1, described straight-run naphtha raw material is carried out to catalytic pyrolysis, difference is, closes with Fischer-TropschBecome oil (character is as shown in table 2) as promoter component. The main operating condition of experiment and the results are shown in table 4.
Embodiment 3
The present embodiment is used for illustrating described naphtha catalytic cracking method of the present invention.
According to the method for embodiment 1, described straight-run naphtha raw material is carried out to catalytic pyrolysis, difference is to use anhydrous secondAlcohol (purity is 99.8 % by weight, purchased from Beijing lark prestige Science and Technology Ltd.) is as promoter component. The main operation bar of experimentPart and the results are shown in table 4.
Embodiment 4
The present embodiment is used for illustrating described naphtha catalytic cracking method of the present invention.
According to the method for embodiment 1, described straight-run naphtha raw material is carried out to catalytic pyrolysis, difference is to use shale oil(character is as shown in table 2) is as promoter component. The main operating condition of experiment and the results are shown in table 5.
Embodiment 5
The present embodiment is used for illustrating described naphtha catalytic cracking method of the present invention.
According to the method for embodiment 1, described straight-run naphtha raw material is carried out to catalytic pyrolysis, difference is to use acetone(it is pure that purity is greater than the analysis of 99.5 % by weight, purchased from Beijing Chemical Plant) is as promoter component. Experiment main operating condition andThe results are shown in table 5.
Embodiment 6
The present embodiment is used for illustrating described naphtha catalytic cracking method of the present invention.
According to the method for embodiment 1, described straight-run naphtha raw material is carried out to catalytic pyrolysis, difference is to use capraldehyde(purity is 96 % by weight, purchased from Beijing lark prestige Science and Technology Ltd.) is as promoter component. Experiment main operating condition andThe results are shown in table 5.
Embodiment 7
The present embodiment is used for illustrating described naphtha catalytic cracking method of the present invention.
According to the method for embodiment 1, described straight-run naphtha raw material is carried out to catalytic pyrolysis, difference is to use dodecaneAcid (purity is 99 % by weight, purchased from Beijing lark prestige Science and Technology Ltd.) is as promoter component. The main operating condition of experimentWith the results are shown in table 5.
Table 1
| The character of straight-run naphtha | |
| Density (20 DEG C), gram per centimeter3 | 0.7358 |
| Vapour pressure, kPa | 50.0 |
| Group composition, % by weight |
| Alkane | 51.01 |
| Cycloalkane | 38.24 |
| Alkene | 0.12 |
| Aromatic hydrocarbons | 10.52 |
| Boiling range, DEG C | |
| IBP | 46 |
| 10％ | 87 |
| 30％ | 107 |
| 50% | 120 |
| 70％ | 133 |
| 90％ | 149 |
| 95% | 155 |
Table 2
| Promoter component | Reduced crude | Fischer-Tropsch synthesis oil | Shale oil |
| Density (20 DEG C), gram per centimeter3 | 0.8950 | 0.8060 | 0.8560 |
| Element composition, % by weight | |||
| C | 86.92 | 85.18 | 86.32 |
| H | 13.08 | 14.47 | 13.66 |
| O | - | 0.35 | - |
| Boiling range, DEG C | |||
| IBP | 317 | 268 | 326 |
| 10％ | 393 | 391 | 378 5 --> |
| 30％ | 456 | 465 | 399 |
| 50% | 533 | 521 | 421 |
| 70％ | - | 584 | 448 |
| 90% | - | 652 | 499 |
Table 3
| Project | Data |
| Chemical composition, % by weight | |
| Al2O3 | 46.3 |
| Na2O | 0.04 |
| Fe2O3 | 0.27 |
| Physical property | |
| Specific area, rice2/ gram | 152 |
| Pore volume, centimetre3/ gram | 0.24 |
| Apparent density, gram per centimeter3 | 0.86 |
| Micro-activity, % | 64 |
Table 4
Table 5
By finding out after the experimental result contrast of embodiment 1-7 in table 4 and table 5 and comparative example 1, urge at existing naphthaChange on the basis of preparing low-carbon olefin by conversion technology, method provided by the invention can obtain higher conversion ratio (conversion ratio=100-gasoline yield-diesel yield) and ethene, productivity of propylene; And low value-added hydrogen+methane+ethane productive rate reduces. With sameCompare Deng the comparative example of not injecting promoter component under reaction condition, conversion ratio and productivity of low carbon olefin hydrocarbon are significantly increased; WhereinConversion ratio has improved more than 15 percentage points, and ethene and productivity of propylene have improved respectively 7.27～9.47 percentage points and 10.56～11.46 percentage points.
By finding out after the experimental result contrast of embodiment 1-7 in table 4 and table 5 and comparative example 2, urge at existing naphthaChange on the basis of preparing low-carbon olefin by conversion technology, method provided by the invention adopts relatively low steam injection rate stillCan obtain higher ethene, productivity of propylene, meanwhile, the productive rate of low value-added hydrogen+methane+ethane and coke reduces, itsMiddle ethene, productivity of propylene have improved respectively 2.52～4.72 percentage points and 9.93～10.83 percentage points.
Claims (8)
1. a naphtha catalytic cracking method, the method comprises: under catalytic pyrolysis condition, in the existence of promoter componentUnder, feed naphtha is contacted with catalytic cracking catalyst, wherein, described promoter component is for compared with described feed naphthaCan on the surface of described catalytic cracking catalyst, preferentially adsorb and/or the material of preferential reaction; Described promoter component isArtificial oil and/or organic oxygen-containing compound; Artificial oil is synthetic through Fischer-Tropsch by least one in coal, natural gas or pitchThe distillate arriving; Organic oxygen-containing compound is selected from the ether of C2～C6, ketone, the aldehyde of C1～C36 and the carboxylic acid of C1～C36 of C3～C5In at least one.
2. method according to claim 1, wherein, with respect to the consumption of the described feed naphtha of 100 weight portions, described inThe consumption of promoter component is 0.01-30 weight portion.
3. method according to claim 2, wherein, with respect to the consumption of the described feed naphtha of 100 weight portions, described inThe consumption of promoter component is 0.05-15 weight portion.
4. method according to claim 1, wherein, described catalytic pyrolysis condition comprises: temperature is 500-750 DEG C, the timeFor 0.2-10 second, agent weight of oil is than being 6-80.
5. method according to claim 4, wherein, described catalytic pyrolysis condition comprises: temperature is 560-690 DEG C, the timeFor 0.5-5 second, agent weight of oil is than being 20-40.
6. method according to claim 1, wherein, described catalytic cracking catalyst contains molecular sieve, heat-resisting inorganic oxideThing and optional clay, taking the gross weight of described catalytic cracking catalyst as benchmark, the content of described molecular sieve is that 5-60 is heavyAmount %, the content of described heat-resistant inorganic oxide is 40-95 % by weight, the content of described clay is 0-70 % by weight.
7. method according to claim 6, wherein, described molecular screening is from ZSM molecular sieve, ZRP molecular sieve, ZSP moleculeIn the molecular sieve that sieve, SAPO molecular sieve, beta-molecular sieve and above-mentioned molecular sieve obtain after physics and/or chemical method processingAt least one; Described heat-resistant inorganic oxide is silica and/or alundum (Al2O3); Described clay be kaolin, ball clay,At least one in imvite, diatomite, rectorite, hydrotalcite, bentonite and laminated clay column.
8. method according to claim 1, wherein, described method is comprising the catalysis of reactor, settler and stripperIn cracker, implement, feed naphtha and catalytic cracking catalyst carry out catalytic cracking reaction in described reactor, obtainThe mixture that contains oil gas and carbon deposited catalyst enters in settler and carries out sedimentation separation, and isolated carbon deposited catalyst enters vapourCarry in device and carry out stripping, the regenerated catalyst obtaining through stripping is turned back in reactor and is followed by regenerated catalyst lineRing uses, and wherein, described promoter component is in described regenerated catalyst line, described reactor, described settler and instituteAt least one place stating in stripper adds.
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| CN1986505A (en) * | 2005-12-23 | 2007-06-27 | 中国石油化工股份有限公司 | Catalytic conversion process with increased low carbon olefine output |
| CN101892067A (en) * | 2010-07-22 | 2010-11-24 | 中国石油天然气股份有限公司 | Method for promoting heavy oil catalytic pyrolysis and improving propylene yield and selectivity |
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| CN1986505A (en) * | 2005-12-23 | 2007-06-27 | 中国石油化工股份有限公司 | Catalytic conversion process with increased low carbon olefine output |
| CN101892067A (en) * | 2010-07-22 | 2010-11-24 | 中国石油天然气股份有限公司 | Method for promoting heavy oil catalytic pyrolysis and improving propylene yield and selectivity |
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